MOF++技术用于贵金属催化剂制备、机理和催化性能研究

In recent years, MOFs composites have been widely used in catalytic research because of their synergistic effects, and have become an important new direction in the research of MOFs. However, there are some problems that need to be solved, such as the addition of stabilizer that will seriously affects the performance of the catalyst, the lack of general and rapid preparation method for monodisperse noble metal nanoparticles, and also the lack of a simple and common strategy for controlling the size of nanoparticles, as well as the interfacial interaction between nanoparticles and MOFs that needs to be strengthened. In view of these problems, we propose to solve the above problems by a kind of MOF++ technology. The specific research contents include: exploring a new method of preparing monodisperse noble metal nanoparticles with no stabilizer and adjustable size by spray technology, which presents a "+" method; in view of our recent development of surface reaction technology, preparing dispersed nanoparticles@MOF composite by coprecipitation, which presents another "+" method; revealing the preparation mechanism of noble metal nanoparticles and composite materials and establishing the best preparation technology through a series of characterization; carrying out the application of such composite materials in selective hydrogenation reaction, and thus revealing the correlation law and structure-activity relationship.

近年来，MOFs复合材料因其协同效应而被广泛应用于催化研究，成为MOFs研究的重要新方向，其虽然表现出良好的应用前景，但也存在一些急需解决的难题如稳定剂的加入严重影响催化剂的性能、单分散贵金属纳米粒子的通用和快速制备、简单且通用的纳米粒子尺寸控制策略、纳米粒子在MOFs负载体上的再次团聚、MOFs与纳米粒子的界面相互作用需加强等。针对这些难题，本项目在前期研究基础上，拟通过一种MOF++技术解决上述难题，具体研究内容包括：探索以喷雾技术制备无稳定剂加入且尺寸可调的单分散贵金属纳米粒子的新方法，此为一“+”；鉴于我们最近发展的表面反应技术，以共沉淀的方式制备分散负载的贵金属纳米粒子@MOFs复合材料，此为另一“+”；通过系列表征，揭示贵金属纳米粒子和复合材料的制备机理和建立其最佳制备工艺技术；研究所制备复合材料在选择性加氢反应方面的应用，并揭示相关规律和构效关系。

MOFs复合材料因其协同效应而被广泛应用于催化研究，成为MOFs研究的重要新方向，其虽然表现出良好的应用前景，但也存在一些急需解决的难题如稳定剂的加入严重影响催化剂的性能、单分散贵金属纳米粒子的通用和快速制备、简单且通用的纳米粒子尺寸控制策略、纳米粒子在MOFs负载体上的再次团聚、MOFs与纳米粒子的界面相互作用需加强等。针对这些难题，本项目在前期研究基础上，首先探索了喷雾技术制备无稳定剂加入且尺寸可调的单分散贵金属纳米粒子的新方法，制备的单分子散铂纳米粒子尺寸为2.4 nm左右，且可以至少稳定两个星期以上， 然后探索了原位化学还原合成银与钯纳米粒子，其尺寸在20 nm 和2 nm左右。在然后通过我们最近发展的表面反应技术，以共沉淀的方式制备将制备贵金属纳米粒子负载到MOF载体上，成功实现了纳米粒子@三氧化二铁@MOF多层复合材料，并通过一系列表征，详细揭示了贵金属纳米粒子和复合材料的制备机理与最佳制备工艺技术。最后申请人探索了所制备复合材料在气体分离与选择性加氢反应方面的应用，并详细揭示了相关规律和构效关系，为进一步指导合成纳米粒子@三氧化二铁@MOF多层复合材料以及催化提供翔实数据与理论支撑。